Dielectric composition



. Patented July 2, 19 46 DIELECTRIC comrosrrlon Massimo Baer, Plainiield, N. 1., assignor to Cornell-Dubilier Electric Corporation, South Plainfield, N. 1., a corporation of Delaware No Drawing. Application November 14,

SerialNo. 465,632

2 Claims. (Cl. 252-66) 1 The present invention relates to dielectric compositions and more particularly to liquid dielectric organic compounds. 1

Various halogenated Organic compositions such as chlorinated naphthalene and chlorinated diphenyl have been proposed as dielectrics for transformers, condensers and other electrical apparatus, both for' direct use in the form of liquid insulators surrounding the apparatus contained in a suitable container and by impregnating the liquid dielectrics in the porous spaces of a primary insulator, in particular, a fibrous insulator such as paper, textiles, and other materials.

Whereas chlorinated diphenyl as liquid dielectrics have been used with great success in the past, other halogenated compositions, in particular chlorinated naphthalenes, have not'been satisi'actory due to their poor dielectric and other electrical properties.

An object of the invention is to provide animproved dielectric composition of the above character and a novel method of preparing the same.

A more specific object is the provision of a new process of transforming ordinary liquid chlorinated naphthalenes possessing poor dielectric properties into compositions of high dielectric and other electrical properties.

With the foregoing and otherobjects in view, as will appear hereafter, the dielectric composition according to theinvention comprises substantially a condensation product or polymer of chlorinated naphthalene, in particular the lower mers obtained by the invention ar the following: A high dielectric constant subject to relatively small variations within a substantial temperature range. According to tests made, the dielectric constants observed were from 4.2 to 4.8 Over a temperature range from C. to 100 C. The dielectric constant at C. ofimpregnated kraft paper was found to be about'5.3.

Another advantage reside: in a low power factor .for electrical condensersimpregnated with the dielectric according to the invention, said power factor being subject to small variations within a substantial temperature range. According to experiments made, the power factor at 1000 cycles was found to range from .2 to .3% at room temperature and from .5 to .6% at a temperature of 100C.

Another characteristic of the dielectric composition obtained by the invention is due to its high insulation resistance.v The latter, according to measurements made, was found to be about 12 megohms per microfarad for a paper condenser employing kraft paper impregnated with the novel dielectric composition according to the 25 invention.

chlorinatednaphthalenes, and formaldehyde or any other compound generating formaldehyde.

One method of carrying'out the invention consists in condensing the lower naphthalenes such as monochloro naphthalene, dichloronaphthalene and trichloro naphthalene or a mixture thereof in various proportions with formaldehyde preferably in the presence of a catalyst. In a preferred embodiment, the catalyst consists of phosphoric anhydride' dissolved in 96% sulphuric acid, The presence of this catalyst substantially increases the rate of condensation and wa found to be indispensable in mixtures involving large portions of dichloro naphthalene and trichloro naphthalene.

By the employment of the above'process, liquid chlorinated naphthalenes which normally POS'. sess poor dielectric and other electrical' properties maybe transformed into naphthalenepolymers or resinous condensation products forming high grade liquid dielectric materials.

Among the many advantages and favorable properties of the chlorinated naphthalene poly- Still another advantage of the new dielectric composition is due to its high breakdown voltage. The latter, according totests made, was found tobe about 3,850 volts in case of direct currentfor a condenser containing three layers of .003 kraft tric materials at present being used as dielectric or insulating compounds such as chlorinated diphenyl and others.

The following is a preferred method; presented by way of example, of practicing the invention. The reagents or initial ingredients used are as follows:

1. One moi of a mixtureof chlorinated naph- 'thalenes, for example a mixture composed of monochloro naphthalene, 30% dichloro naphthalene and 10% trichloro naphthalene; 7

'2. .5? mols of formaldehyde;

3. 96% sulphuric acid in such quantity as to obtain a concentration of 72% sulphuric acid and 28% water;'and

4. Phosphoric anhydride, about 9% of f 3 I weight of the 96% sulphuric acid used and being dissolved in the acid with the aid of heat if needed.

In carrying out the process, one mol of the mixture of chlorinated naphthalenes is stirred with .57 mols of a 37% solution of formaldehyde and heated to 75 C.

The formaldehyde solution may be a U. S. P.

grade containing as active ingredients 37% formaldehyde and as inert ingredients methanol and 53% water. However, any other formaldehyde solution of different. concentration may 1 be used if a sulphuric acid concentration of 72% 1 is maintained. -Methanol is by no means needed for a successful condensation and serves the purpose to avoid separation of some paraformaldehyde from the solutionon long standing.

To this mixture, while being vigorously stirred,

is added the acid mixture in small proportions and during an interval of 1.5 hours. The temperature during this period is kept constant at about 78 to 80 C.

By the addition of 96% sulphuric acid in such quantity as to obtain a concentration of 72% sulphuric acid and 28% water is meant-that, taking into account the water contained in the formaldehyde solution arid the water contained in the 96% sulphuric acid, there is added such a quantity of sulphuric acid as to give a com- I bined concentration of 72% sulphuric acid and 28% water. the final acid concentration which will be rel duced by the water produced during the reaction.

This does not take into account As an example, if a formaldehyde solution is used containing 1'7 grams (37%) of formaldehyde, 4.6 grams (10%) methanol and 24.4 grams (53%) grams of solution, the amount of water X to be added to obtain a combined concentration of 72% sulphuric acid, making altogether 46 sulphuric acid and 28% water will be determined by the following formula:

By determining X, it followsthat 73 grams of 96% sulphuric acid are required to obtaina final acid concentration of 72%.

When the admixture of the acid has been completed, the mass is stirred, for about 3.5 more hours at a temperature of 80 to 85 C. The resinous condensation product or naphthalene polymer formed during the reaction is then separated 4 thalene polymers obtained in the foregoing manwhich comprises the steps of mixing 1 mol of a nor may be further improved and purified by the use of small quantities of activated alumina as w an absorbing agent. The composition has a pale yellow color and contains about 65% solid material and volatile material.

While the invention has been described in terms of its specific embodiment, it is to be understood that it is of a broad application and is to be limited only by the scope of the appended claims. p

I claim: 1. A method of producing a liquid dielectric mixture of the lower chlorinated naphthalenes with .57 mol of a 37% solution of formaldehyde,

heating the mixture to 75 C., stirring the mixture and adding, in small portions. in the interval of about-1.5 hours a solution of 96% sulphuric acidand phosphoric anhydride while maintaining the temperature of the mixture at 78 to 80 C., stirring the mixture for 3.5 more hours at 80 to 85 C. 'to produce a naphthalene-formaldehyde polymer, and segregating the naphthalene polymer from said mixture.

2. A method of producing a liquid dielectric 4 which comprises the steps of mixing 1 mol of a mixture of monochloro naphthalene, 30% dichloro naphthalene and 10% trichloro naphthalene with .57 mol of a 37% solution of formaldehyde, heating the mixture to 0., stirring the mixture and adding, in j small portions, in the interval of 1.5 hours a solution of 96% sulphuric acid .and phosphoric anhydride while maintaining the temperature at 78 to 80 0., stirring the mixture for 3.5 more hours at 80 to C.-, and

segregating by'means of a solvent the naphthalene-formaldehyde polymer formed from said mixture.

- I MASSIMO BAER. 

